Long-Term Field Characterization of Tapered Element Oscillating Microbalance and Modified Tapered Element Oscillating Microbalance Samplers in Urban and Rural New York State Locations

Abstract

Long-term field comparisons of continuous and integrated filter measurements of mass concentrations of par-ticulate matter (PM) with an aerodynamic diameter less than or equal to 2.5 μm (PM_2.5) were performed at rural and urban sites in New York State. Two versions of the continuous tapered element oscillating microbalance (TEOM) mass monitor are deployed at each site, in addition to Federal Reference Method filter samplers. Data are grouped into monthly averages to retain and demonstrate seasonal differences. Strong seasonal dependence is observed—the TEOM monitors with the heated sensors are biased systematically low with respect to the Federal Reference Method measurements during the cold season. For the rural site, the average bias for the sample equilibration system (SES)-equipped and standard TEOM monitors is 14 and 24%, respectively. At this location, the TEOM monitor measurements were biased low for all 34 months. For the urban site, the average bias for the SES and standard TEOM monitors is 8 and 18%, respectively. At this location, the TEOM monitor measurements are as likely to be biased high as low during the warm-season months. The hour averaged data from the two versions of the TEOM monitor are also compared, and also indicate that the SES-equipped version of the TEOM monitor captures 7-11% more PM_2.5 mass at these locations.     

Adjusting tapered element oscillating microbalance data for comparison with Federal Reference Method PM2.5 measurements in region 5

Continuous monitoring of particulate matter (PM) with a diameter less than 2.5 microm (PM2.5) is quickly gaining acceptance as an alternative means of measuring fine PM in the United States. For this project, data were taken from all monitoring sites within Region 5 that used the tapered element oscillating microbalance (TEOM) for PM2.5 and had a collocated Federal Reference Method (FRM) monitor. Scatter plots of TEOM versus FRM show that for a significant fraction of the observations, an independent factor causes the TEOM to underestimate the FRM value. This underestimation appears to increase as temperature decreases. For this analysis, a linear relationship was fit to the TEOM versus FRM data, allowing a break or knot in the relationship, modeled as a change of slope, at a site-specific temperature. To test whether the models are adequate for adjusting future measurements, models were also developed using the first year of data only, and the remaining observations were used to test the durability of the relationships. For all but one monitor in Minnesota, the models developed for each site had consistently high R2s, were predictive of future measurements, and could be used to derive "FRM-like" results from the TEOM measurements. The temperature knots fitted by the model for individual sites ranged from 12.9 to 20.6 degrees C. Data from all six sites in the state of Michigan were also combined to determine if a single model could be developed for the entire state. While the single model for the state of Michigan worked reasonably well, some of the predicted concentrations at individual sites were systematically underestimating the observed concentrations on more polluted days. The same conclusion was drawn for a Region 5-wide model. This approach was also found to work very well for six individual TEOM monitors in New York State.     

Field evaluation of particulate matter measurements using tapered element oscillating microbalance in a layer house

The tapered element oscillating microbalance (TEOM) is one type of continuous ambient particulate matter (PM) monitor. Adsorption and desorption of moisture and semivolatile species may cause positive or negative artifacts in TEOM PM mass measurement. The objective of this field study was to investigate possible uncertainties associated with TEOM measurements in the poultry operation environment. For comparisons of TEOM with filter-based gravimetric method, four instruments (TEOM-PM10, low-volume PM10 sampler TEOM-PM2.5, and PM2.5 speciation sampler) were collocated and tested inside a poultry house for PM2.5 and PM10 (PM with aerodynamic equivalent diameter < or =2.5 and < or =10 microm, respectively) measurements. Fifteen sets of 24-hr PM10 concentrations and 13 sets of 24-hr PM2.5 measurements were obtained. Results indicate that compared with filter-based gravimetric method, TEOM gave significantly lower values of both PM10 and PM2.5 mass concentrations. For PM10, the average ratio of TEOM to the gravimetric method was 0.936. For PM2.5, the average ratio of TEOM to the gravimetric method was 0.738. Particulate matter in the poultry houses possibly contains semivolatile compounds and moisture due to high levels of relative humidity (RH) and gas pollutants. The internal heating mechanism of the TEOM may cause losses in mass through volatilization. To investigate the effects of TEOM settings on concentration measurements, the heaters of two identical TEOMs were set at 50 degrees C, 30 degrees C, or no heating at all. They were collocated and tested for total suspended particle (TSP), PM10, and PM25 measurements in layer house for 6 weeks. For all TSR PM10, and PM2.5 measurements, the internal TEOM temperature setting had a significant effect (P < 0.05). Significantly higher PM mass concentrations were measured at lower temperature settings. The effects of environmental (i.e., temperature, RH, NH3 and CO2 concentrations) and instrumental (i.e., filter loading and noise) parameters on PM measurements were also assessed using regression analysis.     

New York State urban and rural measurements of continuous PM2.5 mass by FDMS, TEOM, and BAM

Field evaluations and comparisons of continuous fine particulate matter (PM2,5) mass measurement technologies at an urban and a rural site in New York state are performed. The continuous measurement technologies include the filter dynamics measurement system (FDMS) tapered element oscillating microbalance (TEOM) monitor, the stand-alone TEOM monitor (without the FDMS), and the beta attenuation monitor (BAM). These continuous measurement methods are also compared with 24-hr integrated filters collected and analyzed under the Federal Reference Method (FRM) protocol. The measurement sites are New York City (the borough of Queens) and Addison, a rural area of southwestern New York state. New York City data comparisons between the FDMS TEOM, BAM, and FRM are examined for bias and seasonality during a 2-yr period. Data comparisons for the FDMS TEOM and FRM from the Addison location are examined for the same 2-yr period. The BAM and FDMS measurements at Queens are highly correlated with each other and the FRM. The BAM and FDMS are very similar to each other in magnitude, and both are approximately 25% higher than the FRM filter measurements at this site. The FDMS at Addison measures approximately 9% more mass than the FRM. Mass reconstructions using the speciation trends network filter data are examined to provide insight as to the contribution of volatile species of PM2.5 in the FDMS mass measurement and the fraction that is likely lost in the FRM mass measurement. The reconstructed mass at Queens is systematically lower than the FDMS by approximately 10%.     

Development of a Sample Equilibration System for the TEOM Continuous PM Monitor

ABSTRACT

In recent years, scientific discussion has included the influence of thermodynamic conditions (e.g., temperature, relative humidity, and filter face velocity) on PM retention efficiency of filter-based samplers and monitors. Method-associated thermodynamic conditions can, in some instances, dramatically influence the presence of particle-bound water and other light-molecular-weight chemical components such as particulate nitrates and certain organic compounds. The measurement of fine particle mass presents a new challenge for all PM measurement methods, since a relatively greater fraction of the mass is semi-volatile.

The tapered element oscillating microbalance (TEOM) continuous PM monitor is a U.S. Environmental Protection Agency (EPA) PM₁₀ equivalent method (EQPM-1090-079). Several hundred of these monitors are deployed throughout the United States. The TEOM monitor has the unique characteristic of providing direct PM mass measurement without the calibration uncertainty inherent in mass surrogate methods. In addition, it provides high-precision, near-real-time continuous data automatically. Much attention has been given to semi-volatile species retention of the TEOM method.

While using this monitor, it is desirable to maintain as low an operating temperature as practical and to remove unwanted particle-bound water. A new sample equilibration system (SES) has been developed to allow conditioning of the PM sample stream to a lower humidity and temperature level. The SES incorporates a special low-particle-loss Nafion dryer. This paper discusses the configuration and theory of the SES. Performance results include high time-resolved PM_2.5 data comparison between a 30 °C sample stream TEOM monitor with SES and a standard 50 °C TEOM monitor. In addition, 24-hr integrated data are compared with data collected using an EPA PM_2.5 Federal Reference Method (FRM)-type sampler. The SES is a significant development because it can be applied easily to existing TEOM monitors.     

Laboratory characterization of modified tapered element oscillating microbalance samplers

Laboratory tests with generated aerosols were conducted to test the efficacy of two recent design modifications to the well-established tapered element oscillating microbalance (TEOM) continuous particulate matter (PM) mass monitor. The two systems tested were the sample equilibration system-equipped TEOM monitor operating at 30 degrees C, which uses a Nafion dryer as part of the sample inlet, and the differential TEOM monitor, which adds a switched electrostatic precipitator and uses a self-referencing algorithm to determine "true PM mass." Test aerosols included ammonium sulfate, ammonium nitrate, sodium chloride, copper (II) sulfate, and mixed aerosols. Aerosols were generated with an atomizer or a vibrating orifice generator and were equilibrated in a 450-L slow flow chamber before being sampled. Relative humidity in the chamber was varied between 10 and 90%, and step changes in humidity were executed while generating aerosol to test the response of the instruments. The sample equilibration system-equipped TEOM monitor does reduce, but not totally eliminate, the sensitivity of the TEOM mass monitor to changes in humidity. The differential TEOM monitor gives every indication of being a very robust technique for the continuous real-time measurement of ambient aerosol mass, even in the presence of semi-volatile particles and condensable gases.     

Improving the correlations of ambient tapered element oscillating microbalance PM2.5 data and SHARP 5030 Federal Equivalent Method in Ontario: A multiple linear regression analysis

Tapered element oscillating microbalances equipped with sample equilibration system (TEOM-SES) used by the province of Ontario for the ambient monitoring of PM_2.5 (particulate matter with an aerodynamic diameter ≤2.5 µm) in its air quality index (AQI) network were collocated with the Synchronized Hybrid Ambient Real-time Particulate monitor (SHARP 5030) at two monitoring sites for a period spanning approximately 2 years to determine the similarities and differences between the measurement outputs of both instrumental systems. Due mainly to mass loss observed with the TEOM-SES in cooler months, the province has recently switched its PM_2.5 instrumentation at all stations in its monitoring network from the TEOM-SES to the SHARP 5030, which has the U.S. Environmental Protection Agency (EPA) Federal Equivalent Method (FEM) Class III designation. Thus, it has become imperative to develop corrections for historical and future TEOM measurements for the purpose of making them more agreeable to the new FEM method. This work details the authors’ multiple linear regression analyses (MLRAs) of particulate matter data from both instrumental monitors, with the inclusion of operational parameters of physicochemical relevance for both cases of transformations of historical TEOM and TEOM measurements to be made in the future. For historical TEOM data, it was observed that the transformations only benefited winter and fall months. Furthermore, comparisons of the transformed historical TEOM data with PM_2.5 concentrations determined from the Federal Reference Method (FRM) sampler at seven locations within the province showed marked improvements over the observed TEOM-FRM comparisons.

Implications:This work provides a path to correcting the historically observed underreporting of particulate mass in winter and fall in Ontario by making the TEOM-based continuous data resemble the new FEM outputs (in this case, more SHARP-like). It is possible that the transformation of mainly winter TEOM data as detailed in this work may potentially lead to revisions in historical annual composite mean PM_2.5 concentrations and total annual number of days PM_2.5 exceeded the Canada-wide Standard (CWS) metric across the province.     

Evaluation and comparison of continuous fine particulate matter monitors for measurement of ambient aerosols

To provide a scientific basis for the selection and use of continuous monitors for exposure and/or health effects studies, and for compliance and episode measurements at strategic locations in the State of New Jersey, we evaluated the performance of seven continuous fine particulate matter (PM2.5) monitors in the present study. Gravimetric samplers, as reference methods, were collocated with realtime instruments in both laboratory and field tests. The results of intercomparison of real-time monitors showed that the two nephelometers used in this study correlated extremely well (r2 approximately 0.97), and two tapered element oscillating monitors (TEOM 1400 and TEOM filter dynamics measurement system [FDMS]) correlated well (r2 > 0.85), whereas two beta gauges displayed a weaker correlation (r2 < 0.6). During a summertime controlled (laboratory) evaluation, the measurements made with the gravimetric method correlated well with the 24-hr integrated measurements made with the real-time monitors. The SidePak nephelometer overestimated the particle concentration by a factor of approximately 3.4 compared with the gravimetric method. During a summertime field evaluation, the TEOM FDMS monitor reported approximately 30% higher mass concentration than the Federal Reference Method (FRM); and the difference could be explained by the loss of semi-volatile materials from the FRM sampler. Results also demonstrated that 24-hr average PM2.5 mass concentrations measured by beta gauges and TEOM (50 degrees C) in winter correlated well with the integrated gravimetric method. Seasonal differences were observed in the performance of the TEOM (50 degrees C) monitor in measuring the particle mass attributed to the higher semi-volatile material loss in the winter weather. In applying the realtime particulate matter monitoring data into Air Quality Index (AQI) reporting, the Conroy method and the 8-hr end-hour average method were both found to be suitable.     

Continuous determination of fine particulate matter mass in the Salt Lake City Environmental Monitoring project: a comparison of real-time and conventional TEOM monitor results

Fine particulate matter (PM2.5) mass was determined on a continuous basis at the Salt Lake City Environmental Protection Agency Environmental Monitoring for Public Awareness and Community Tracking monitoring site in Salt Lake City, UT, using three different monitoring techniques. Hourly averaged PM2.5 mass data were collected during two sampling periods (summer 2000 and winter 2002) using a real-time total ambient mass sampler (RAMS), sample equilibration system (SES)-tapered element oscillating microbalance (TEOM), and conventional TEOM monitor. This paper compares the results obtained from the various monitoring systems, which differ in their treatment of semivolatile material (SVM; particle-bound water, semivolatile ammonium nitrate, and semivolatile organic compounds). PM2.5 mass results obtained by the RAMS were consistently higher than those obtained by the SES-TEOM and conventional TEOM monitors because of the RAMS ability to measure semivolatile ammonium nitrate and semivolatile organic material but not particle-bound water. The SES-TEOM monitoring system was able to account for an average of 28% of the SVM, whereas the conventional TEOM monitor loses essentially all of the SVM from the single filter during sampling. Occasional mass readings by the various TEOM monitors that are higher than RAMS results may reflect particle-bound water, which, under some conditions, is measured by the TEOM but not the RAMS.     

Comparison of measured total suspended particulate matter concentrations using tapered element oscillating microbalance and a total suspended particulate sampler

A comparison of the concentration of the total suspended particulate (TSP) matter measured by the tapered element oscillating microbalance (TEOM) monitor and the isokinetic TSP samplers developed at the University of Illinois was carried out in several types of confinement livestock buildings. In a majority of the measurements done, the dust concentration measured by the TEOM monitor was lower than the University of Illinois at Urbana-Champaign (UIUC) isokinetic TSP sampler; the TEOM monitor tended to underestimate the total dust concentration by as much as 54%. The difference in measurements can be attributed to the sampling efficiency of the TEOM monitor sampling head and the loss of some semivolatile compounds and particle-bound water because of heating of the TEOM monitor sampling stream to 50 degrees C. Although several articles in the literature supported the latter argument, this study did not investigate the effect of heating the sampling stream or the effect of moisture on the relative difference in dust concentration measurements. The model that best describes the relationship between the two methods was site specific, that is, the linear regression model was applicable only to four of the sites monitored. The measured total dust concentration in livestock buildings range from approximately 300 to 4000 microg/m3; a higher correlation coefficient between TEOM-TSP and UIUC-TSP monitors was obtained in swine facilities than those obtained in a laying facility.     

The measurement of fine particulate semivolatile material in urban aerosols

Ammonium nitrate and semivolatile organic material (SVOM) are significant components of fine particles in urban atmospheres. These components, however, are not properly determined with methods such as the fine particulate matter (PM2.5) Federal Reference Method (FRM) or other single filter samplers because of significant losses of semivolatile material (SVM) from particles collected on the filter during sampling. The R&P tapered element oscillating microbalance (TEOM) monitor also does not measure SVM, because this method heats the sample to remove particle bound water, which also results in evaporation of SVM. Recent advances in monitoring techniques have resulted in samplers for both integrated and continuous measurement of total PM2.5, including the particle concentrator-Brigham Young University organic sampling system (PC-BOSS), the real-time total ambient mass sampler (RAMS), and the R&P filter dynamics measurement system (FDMS) TEOM monitor. Results obtained using these samplers have been compared with those obtained with either a PM2.5 FRM sampler or a TEOM monitor in studies conducted during the past five years. These studies have shown the following: (1) the PC-BOSS, RAMS, and FDMS TEOM are all comparable. Each instrument measures both the nonvolatile material and the SVM. (2) The SVM is not retained on the heated filter of a regular TEOM monitor and is not measured by this sampling technique. (3) Much of the SVM is also lost during sampling from single filter samplers such as the PM2.5 FRM sampler. (4) The amount of SVM lost from single filter samplers can vary from less than one-third of that lost from heated TEOM filters during cold winter conditions to essentially all during warm summer conditions. (5) SVOM can only be reliably collected using an appropriate denuder sampler. (6) A PM2.5 speciation sampler can be easily modified to a denuder sampler with filters that can be analyzed for semivolatile organic carbon (OC), nonvolatile OC, and elemental carbon using existing OC/elemental carbon analytical techniques. The research upon which these statements are based for various urban studies are summarized in this paper.     

An evaluation of the tapered element oscillating microbalance method for measuring diesel particulate emissions

We determined the usefulness of tapered element oscillating microbalances (TEOMs) for researchers and engineers involved with measuring diesel particulate mass. Two different test facilities were used for generating diesel particulates and comparing the TEOM to the commonly used U.S. Environmental Protection Agency (EPA) manual filter method. The EPA method is very labor-intensive and requires long periods of time to complete. The TEOM is an attractive approach because it has the potential to reduce the amount of time and labor required in diesel testing, as well as to provide real-time particulate-mass data that are not obtainable with the EPA method. It was found that the TEOM was a precise and easy-to-operate instrument that could measure the mass concentration (MC) of diesel particulate emissions in real time. Although the TEOM diesel particulate MC measurements were highly correlated with the manual filter measurements, the two techniques were not equivalent because the TEOM consistently reported MC results that were 20-25% lower than those obtained using the manual filter technique. In conclusion, the TEOM can be used to increase test-cell throughput and to measure transient values of diesel particulate emissions at sites performing diesel-engine testing. However, unless EPA is able to certify the TEOM as an equivalent method, it cannot replace the manual filter method for diesel certification work.     

Human Exposure to Sulfates from Coal-Fired Power Plants

Abstract

Increased interest in the health effects of ambient par–ticulate mass (PM) has focused attention on the evaluation of existing mass measurement methodologies and the definition of PM in ambient air. The Rupprecht and Patashnick Tapered Element Oscillating MicroBalance (TEOM^®) method for PM is compared with time–integrated gravimetric (manual) PM methods in large urban areas during different seasons. Comparisons are conducted for both PM₁₀ and PM_2.5 concentrations.

In urban areas, a substantial fraction of ambient PM can be semi–volatile material. A larger fraction of this component of PM₁₀ may be lost from the TEOM–heated filter than the Federal Reference Method (FRM). The observed relationship between TEOM and FRM methods varied widely among sites and seasons. In East Coast urban areas during the summer, the methods were highly correlated with good agreement. In the winter, correlation was somewhat lower, with TEOM PM concentrations generally lower than the FRM. Rubidoux, CA, and two Mexican sites (Tlalnepantla and Merced) had the highest levels of PM₁₀ and the largest difference between TEOM and manual methods.

PM_2.5 data from collocation of 24–hour manual samples with the TEOM are also presented. As most of the semi–volatile PM is in the fine fraction, differences between these methods are larger for PM_2.5 than for PM₁₀.     

Estimation of ambient PM2.5 concentrations in Maryland and verification by measured values

In 1997, Maryland had no available ambient Federal Reference Method data on particulate matter less than 2.5 microm in aerodynamic diameter (PM23), but did have annual ambient data for PM smaller than 10 microm (PM10) at 24 sites. The PM10 data were analyzed in conjunction with local annual and seasonal zip-code-level emission inventories and with speciated PM2.5 data from four nearby monitors in the IMPROVE network (located in the national parks, wildlife refuges, and wilderness areas) in an effort to estimate annual average and seasonal high PM2.5 concentrations at the 24 PM10 monitor sites operating from 1992 to 1996. All seasonal high concentrations were estimated to be below the 24-hr PM2.5 National Ambient Air Quality Standards (NAAQS) at the sites operating in Maryland between 1992 and 1996. The estimates also indicated that 12 monitor sites might exceed the 3-year annual average PM2.5 NAAQS of 15 microg/m3, but Maryland's air quality shows signs that it has been improving since 1992. The estimates also were compared with actual measurements after the PM2.5 monitor network was installed. The estimates were adequate for describing the chemical composition of the PM2.5, forecasting compliance status with the 24-hr and annual standards, and determining the spatial variations in PM2.5 across central Maryland.     

Air quality measurements from the Fresno Supersite

The Fresno Supersite intends to 1) evaluate non-routine monitoring methods, establishing their comparability with existing methods and their applicability to air quality planning, exposure assessment, and health effects studies; 2) provide a better understanding of aerosol characteristics, behavior, and sources to assist regulatory agencies in developing standards and strategies that protect public health; and 3) support studies that evaluate relationships between aerosol properties, co-factors, and observed health end-points. Supersite observables include in-situ, continuous, short-duration measurements of 1) PM2.5, PM10, and coarse (PM10 minus PM2.5) mass; 2) PM2.5 SO4(-2), NO3-, carbon, light absorption, and light extinction; 3) numbers of particles in discrete size bins ranging from 0.01 to approximately 10 microns; 4) criteria pollutant gases (O3, CO, NOx); 5) reactive gases (NO2, NOy, HNO3, peroxyacetyl nitrate [PAN], NH3); and 6) single particle characterization by time-of-flight mass spectrometry. Field sampling and laboratory analysis are applied for gaseous and particulate organic compounds (light hydrocarbons, heavy hydrocarbons, carbonyls, polycyclic aromatic hydrocarbons [PAH], and other semi-volatiles), and PM2.5 mass, elements, ions, and carbon. Observables common to other Supersites are 1) daily PM2.5 24-hr average mass with Federal Reference Method (FRM) samplers; 2) continuous hourly and 5-min average PM2.5 and PM10 mass with beta attenuation monitors (BAM) and tapered element oscillating microbalances (TEOM); 3) PM2.5 chemical speciation with a U.S. Environmental Protection Agency (EPA) speciation monitor and protocol; 4) coarse particle mass by dichotomous sampler and difference between PM10 and PM2.5 BAM and TEOM measurements; 5) coarse particle chemical composition; and 6) high sensitivity and time resolution scalar and vector wind speed, wind direction, temperature, relative humidity, barometric pressure, and solar radiation. The Fresno Supersite is coordinated with health and toxicological studies that will use these data in establishing relationships with asthma, other respiratory disease, and cardiovascular changes in human and animal subjects.     

Comparison between a personal PM10 sampling head and the tapered element oscillating microbalance (TEOM) system

A new personal PM₁₀ sampling head has been developed by the Institute of Occupational Medicine (IOM), Edinburgh. The purpose of this study was to compare its performance in the field with the accepted fixed-location PM₁₀ sampler, the tapered element oscillating microbalance (TEOM). The comparisons were carried out on three separate occasions during 1997 at each of two city centre locations in the UK. On each occasion two personal IOM PM₁₀ sampling heads were located adjacent to a TEOM monitor and four successive sets of 24-h filter samples were collected. The data was compared with 24-h average TEOM concentrations, calculated as the arithmetic mean of the recorded hourly averages. There was a statistically significant linear relationship between the two types of monitor, although the concentrations from the IOM PM₁₀ samplers were consistently higher than the TEOM data. It is therefore possible to use the regression equations presented in this paper to correct ambient PM₁₀ concentrations measured by either method to equivalent values. Further research is needed to properly understand the reason for the difference between the TEOM and filter samplers.     

The regional nature of PM2.5 episodes in the upper Ohio River Valley

From October 1999 through September 2000, particulate matter (PM) with aerodynamic diameter > or =2.5 microm (PM2.5) mass and composition were measured at the National Energy Technology Laboratory Pittsburgh site, with a particle concentrator Brigham Young University-organic sampling system and a tapered element oscillating microbalance (TEOM) monitor. PM2.5 measurements had also been obtained with TEOM monitors located in the Pittsburgh, PA, area, and at sites in Ohio, including Steubenville, Columbus, and Athens. The PM data from all these sites were analyzed on high PM days; PM2.5 TEOM particulate mass at all sites was generally associated with transitions from locally high barometric pressure to lower pressure. Elevated concentrations occurred with transport of PM from outside the local region in advance of frontal passages as the local pressure decreased. During high-pressure periods, concentrations at the study sites were generally low throughout the study region. Further details related to this transport were obtained from surface weather maps and estimated back-trajectories using the hybrid single-particle Lagrangian integrated trajectory model associated with these time periods. These analyses indicated that transport of pollutants to the Pittsburgh site was generally from the west to the southwest. These results suggest that the Ohio River Valley and possible regions beyond act as a significant source of PM and its precursors in the Pittsburgh area and at the other regional sites included in this study.     

Nonlinear regression adjustments of multiple continuous monitoring methods produce effective characterization of short-term fine particulate matter

This study comprehensively characterizes hourly fine particulate matter (PM(2.5)) concentrations measured via a tapered element oscillating microbalance (TEOM), beta-gauge, and nephelometer from four different monitoring sites in U.S. Environment Protection Agency (EPA) Region 5 (in U.S. states Illinois, Michigan, and Wisconsin) and compares them to the Federal Reference Method (FRM). Hourly characterization uses time series and autocorrelation. Hourly data are compared with FRM by averaging across 24-hr sampling periods and modeling against respective daily FRM concentrations. Modeling uses traditional two-variable linear least-squares regression as well as innovative nonlinear regression involving additional meteorological variables such as temperature and humidity. The TEOM shows a relationship with season and temperature, linear correlation as low as 0.7924 and nonlinear model correlation as high as 0.9370 when modeled with temperature. The beta-gauge shows no relationship with season or meteorological variables. It exhibits a linear correlation as low as 0.8505 with the FRM and a nonlinear model correlation as high as 0.9339 when modeled with humidity. The nephelometer shows no relationship with season or temperature but a strong relationship with humidity is observed. A linear correlation as low as 0.3050 and a nonlinear model correlation as high as 0.9508 is observed when modeled with humidity. Nonlinear models have higher correlation than linear models applied to the same dataset. This correlation difference is not always substantial, which may introduce a tradeoff between simplicity of model and degree of statistical association. This project shows that continuous monitor technology produces valid PM(2.5) characterization, with at least partial accounting for variations in concentration from gravimetric reference monitors once appropriate nonlinear adjustments are applied. Although only one regression technically meets new EPA National Ambient Air Quality Standards (NAAQS) Federal Equivalent Method (FEM) correlation coefficient criteria, several others are extremely close, showing optimistic potential for use of this nonlinear adjustment model in garnering EPA NAAQS FEM approval for continuous PM(2.5) sampling methods.     

Collocated comparisons of continuous and filter-based PM2.5 measurements at Fort McMurray,Alberta, Canada

Collocated comparisons for three PM_2.5 monitors were conducted from June 2011 to May 2013 at an air monitoring station in the residential area of Fort McMurray, Alberta, Canada, a city located in the Athabasca Oil Sands Region. Extremely cold winters (down to approximately ?40°C) coupled with low PM_2.5 concentrations present a challenge for continuous measurements. Both the tapered element oscillating microbalance (TEOM), operated at 40°C (i.e., TEOM₄₀), and Synchronized Hybrid Ambient Real-time Particulate (SHARP, a Federal Equivalent Method [FEM]), were compared with a Partisol PM_2.5 U.S. Federal Reference Method (FRM) sampler. While hourly TEOM₄₀ PM_2.5 were consistently ~20–50% lower than that of SHARP, no statistically significant differences were found between the 24-hr averages for FRM and SHARP. Orthogonal regression (OR) equations derived from FRM and TEOM₄₀ were used to adjust the TEOM₄₀ (i.e., TEOM_adj) and improve its agreement with FRM, particularly for the cold season. The 12-year-long hourly TEOM_adj measurements from 1999 to 2011 based on the OR equations between SHARP and TEOM₄₀ were derived from the 2-year (2011–2013) collocated measurements. The trend analysis combining both TEOM_adj and SHARP measurements showed a statistically significant decrease in PM_2.5 concentrations with a seasonal slope of ?0.15 μg m^?3 yr^?1 from 1999 to 2014.Implications: Consistency in PM_2.5 measurements are needed for trend analysis. Collocated comparison among the three PM_2.5 monitors demonstrated the difference between FRM and TEOM, as well as between SHARP and TEOM. The orthogonal regressions equations can be applied to correct historical TEOM data to examine long-term trends within the network.     

A two-step approach for relating tapered element oscillating microbalance and dichotomous air sampler PM2.5 measurements

A method for transforming continuous monitoring (CM) fine particulate matter (aerodynamic diameter <2.5 μm; PM_2.5) data (i.e., by tapered element oscillating microbalance [TEOM]) obtained from the Canadian National Air Pollution Surveillance (NAPS) program to meet the data quality objective (DQO) of R² > 0.8 against the co-located federal reference method (i.e., dichotomous air sampler) is described. By using a two-step linear regression to account for the effect of the ambient temperature, 16 out of the 23 examined sites met the common model adequacy threshold of R² > 0.8. After the transformation, 20 out of the 23 examined sites met the DQO of R² > 0.7, as recommended by the U.S. Environmental Protection Agency (EPA). A combined two-step statistical approach was also examined and revealed similar results. The methods described herein show that the CM data can be successfully transformed to meet DQOs for representative sites across Canada using year-round (both summer and winter) data.

Implications:This study provides a transformation approach to correct ambient TEOM data against the federal reference method without dividing the ambient data according to warm and cold seasons. This transformation approach will significantly improve the correlation coefficient between TEOM and dichotomous air sampler data. It is possible that TEOM data at many Canadian locations can be transformed to meet the EPA data quality objective, thus making this transformation approach useful for comparisons of ambient PM data across jurisdictions.